Journal
ADVANCED MATERIALS
Volume 32, Issue 8, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201906806
Keywords
hydration effect; neutral electrolytes; Ni-Fe catalysts; oxygen evolution reaction
Categories
Funding
- Ontario Research Fund -Research Excellence Program
- Natural Sciences and Engineering Research Council of Canada
- CIFAR Bio-Inspired Solar Energy program
- International Cooperation Projects of the Ministry of Science and Technology [2014DFE60170]
- National Natural Science Foundation of China [21875042, 61474065, 61674084]
- Tianjin Research Key Program of Science and Technology [18ZXJMTG00220]
- 111 Project [B16027]
- Fundamental Research Funds for the Central Universities
- Ministry of Science and Technology [2016YFA0203302]
- Science and Technology Commission of Shanghai Municipality [18QA1400800]
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning
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Oxygen evolution reaction (OER) catalysts that function efficiently in pH-neutral electrolyte are of interest for biohybrid fuel and chemical production. The low concentration of reactant in neutral electrolyte mandates that OER catalysts provide both the water adsorption and dissociation steps. Here it is shown, using density functional theory simulations, that the addition of hydrated metal cations into a Ni-Fe framework contributes water adsorption functionality proximate to the active sites. Hydration-effect-promoting (HEP) metal cations such as Mg2+ and hydration-effect-limiting Ba2+ into Ni-Fe frameworks using a room-temperature sol-gel process are incorporated. The Ni-Fe-Mg catalysts exhibit an overpotential of 310 mV at 10 mA cm(-2) in pH-neutral electrolytes and thus outperform iridium oxide (IrO2) electrocatalyst by a margin of 40 mV. The catalysts are stable over 900 h of continuous operation. Experimental studies and computational simulations reveal that HEP catalysts favor the molecular adsorption of water and its dissociation in pH-neutral electrolyte, indicating a strategy to enhance OER catalytic activity.
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